Gap and Grain-Boundary Inventories of Cs, Tc, and Sr in Spent LWR Fuel

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ABSTRACTSoluble radionuclides concentrated within the gap and grain-boundary regions of spent fuel could dissolve relatively rapidly were the waste container to fail and the fuel to be contacted by water in a geologic repository. To provide an estimate of the quantities of radionuclides that may be rapidly released, fractional inventories of Cs, Tc, and Sr concentrated within the fuel/cladding gap region have been measured for U.S. LWR spent fuels with fission gas release (FGR) values ranging from 0.25% to 18%. Separate measurements of the grain-boundary inventories of Cs, Tc, and Sr have been made for the same fuels. The Cs gap inventories were generally found to be about one fourth of the FGR values. The Cs grain-boundary inventories were generally less than 1% of the total Cs inventories and were not strongly correlated with FGR. Both the gap and grain-boundary inventories of Tc and Sr were near the detection limits of the methods used, less than 0.2% of the total inventories of these elements. However, some of the Tc may reside at the grain boundaries in the form of relatively insoluble metallic particles and not be detected by these experiments. Data obtained by comparing the dissolution behavior of fuel fragments with that of fuel grains were used to estimate the dissolution rate of Cs from the grain boundaries of one of the fuels. Surface-area normalized dissolution rates determined for fuel fragments in these same tests exceeded those determined for grains. A likely explanation is that the estimated fragment surface area did not take into account the “effective” grain-boundary surfaces.